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烷基咪唑基介孔有机硅的合成与表征:用于固定高钌酸盐(RuO4-)的多功能主体在醇的有氧氧化中的应用。

Synthesis and characterization of alkyl-imidazolium-based periodic mesoporous organosilicas: a versatile host for the immobilization of perruthenate (RuO4-) in the aerobic oxidation of alcohols.

机构信息

Department of Chemistry, Institute for Advanced Studies in Basic Sciences, PO Box 45195-1159, Gava zang Zanjan, 45137-6731, Iran.

出版信息

Chemistry. 2012 Oct 15;18(42):13520-30. doi: 10.1002/chem.201200380. Epub 2012 Sep 3.

DOI:10.1002/chem.201200380
PMID:22945297
Abstract

The preparation and characterization of a set of periodic mesoporous organosilicas (PMOs) that contain different fractions of 1,3-bis(3-trimethoxysilylpropyl)imidazolium chloride (BTMSPI) groups uniformly distributed in the silica mesoporous framework is described. The mesoporous structure of the materials was characterized by powder X-ray diffraction, transmission electron microscopy, and N(2) adsorption-desorption analysis. The presence of propyl imidazolium groups in the silica framework of the materials was also characterized by solid-state NMR spectroscopy and diffuse-reflectance Fourier-transform infrared spectroscopy. The effect of the BTMSPI concentration in the initial solutions on the structural properties (including morphology) of the final materials was also examined. The total organic content of the PMOs was measured by elemental analysis, whereas their thermal stability was determined by thermogravimetric analysis. Among the described materials, it was found that PMO with 10% imidazolium content is an effective host for the immobilization of perruthenate through an ion-exchange protocol. The resulting Ru@PI-10 was then employed as a recyclable catalyst in the highly efficient aerobic oxidation of various types of alcohols.

摘要

描述了一组周期性介孔有机硅(PMO)的制备和表征,这些 PMO 中均匀分布着不同比例的 1,3-双(3-三甲氧基硅丙基)咪唑𬭩氯化物(BTMSPI)基团,分布在硅介孔骨架中。通过粉末 X 射线衍射、透射电子显微镜和 N2 吸附-脱附分析对材料的介孔结构进行了表征。通过固态 NMR 光谱和漫反射傅里叶变换红外光谱也对材料硅骨架中存在的丙基咪唑基团进行了表征。还考察了初始溶液中 BTMSPI 浓度对最终材料结构性质(包括形态)的影响。通过元素分析测量 PMO 的总有机含量,通过热重分析测定其热稳定性。在所描述的材料中,发现 PMO 中含有 10%的离子含量是通过离子交换法固定高钌酸盐的有效主体。所得的 Ru@PI-10 随后被用作高效有氧氧化各种醇的可回收催化剂。

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